Although CsPbBrxI3−x quantum dots (QDs) have wide prospects for application in red light-emitting diodes (LEDs) due to their superior optoelectronic properties, the presence of defects and insulating long-chain ligands severely limits their luminescence performance. A novel strategy of spinning-coated CsPbBrxI3−x QDs on a PEABr or PEAI modified layer is designed to obtain red LEDs with efficient performance. The systematic studies on the structural evolution and optoelectronic properties of CsPbBrxI3−x QDs are discussed. The structural stability and electrical conductivity of CsPbBrxI3−x QDs are significantly improved because the halogen vacancies and insulating long-chain ligands (oleic acid and oleylamine) in CsPbBrxI3−x QDs are passivated and replaced by halogens and short-chain PEA from PEAX (X = Br and I), respectively. Modifying PEABr and PEAI obviously enhances the maximum external quantum efficiency (EQEmax) of CsPbBrxI3−x LEDs from 1.6 % to 11.7 %, and 14.9 %, respectively. Additionally, the electroluminescence (EL) spectral stability and useful life of LEDs are also ameliorated. The interfacial layer formed by the modified solution during the fabrication process of LEDs can effectively passivate the defects in QD films and improve the performance of LEDs. This preparation method is simple and easy to operate, which facilitates the design of efficient and stable QD-LEDs.